The behavior of polyatomic molecules around their equilibrium positions can be regarded as that of quantum-coupled anharmonic oscillators. Solving the corresponding Schrödinger equations enables the interpretation or prediction of the experimental spectra of molecules. In this study, we developed a novel approach for solving the excited states of anharmonic vibrational systems. The normal coordinates of the molecules are transformed into new coordinates through a normalizing flow parameterized by a neural network. This facilitates the construction of a set of orthogonal many-body variational wavefunctions. This methodology has been validated on an exactly solvable 64-dimensional coupled harmonic oscillator, yielding numerical results with a relative error of 10−6. The neural canonical transformations are also applied to calculate the energy levels of two specific molecules, acetonitrile (CH3CN) and ethylene oxide (C2H4O). These molecules involve 12 and 15 vibrational modes, respectively. A key advantage of this approach is its flexibility concerning the potential energy surface, as it requires no specific form. Furthermore, this method can be readily implemented on large-scale distributed computing platforms, making it easy to extend to investigating complex vibrational structures.
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14 July 2024
Research Article|
July 09 2024
Neural canonical transformations for vibrational spectra of molecules Available to Purchase
Qi Zhang
;
Qi Zhang
a)
(Methodology, Writing – original draft, Writing – review & editing)
1
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
a)Author to whom correspondence should be addressed: [email protected]
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Rui-Si Wang
;
Rui-Si Wang
(Methodology, Writing – original draft, Writing – review & editing)
1
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Lei Wang
Lei Wang
b)
(Methodology, Writing – original draft, Writing – review & editing)
1
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
3
Songshan Lake Materials Laboratory
, Dongguan, Guangdong 523808, China
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Qi Zhang
1,a)
Rui-Si Wang
1,2
Lei Wang
1,3,b)
1
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
3
Songshan Lake Materials Laboratory
, Dongguan, Guangdong 523808, China
a)Author to whom correspondence should be addressed: [email protected]
b)
Electronic mail: [email protected]
J. Chem. Phys. 161, 024103 (2024)
Article history
Received:
March 20 2024
Accepted:
June 19 2024
Citation
Qi Zhang, Rui-Si Wang, Lei Wang; Neural canonical transformations for vibrational spectra of molecules. J. Chem. Phys. 14 July 2024; 161 (2): 024103. https://doi.org/10.1063/5.0209255
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